EP0775107B1 - Preparation of o-(2-hydroxyalkyl) oximes - Google Patents

Preparation of o-(2-hydroxyalkyl) oximes Download PDF

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Publication number
EP0775107B1
EP0775107B1 EP95930419A EP95930419A EP0775107B1 EP 0775107 B1 EP0775107 B1 EP 0775107B1 EP 95930419 A EP95930419 A EP 95930419A EP 95930419 A EP95930419 A EP 95930419A EP 0775107 B1 EP0775107 B1 EP 0775107B1
Authority
EP
European Patent Office
Prior art keywords
oxime
ketoxime
catalyst
carbonate
salts
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP95930419A
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German (de)
English (en)
French (fr)
Other versions
EP0775107A1 (en
Inventor
Albrecht Harreus
Norbert Götz
Harald Rang
Horst Hartmann
Jürgen Mohr
Eugen Gehrer
Günter Lauth
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BASF SE
Original Assignee
BASF SE
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Filing date
Publication date
Application filed by BASF SE filed Critical BASF SE
Publication of EP0775107A1 publication Critical patent/EP0775107A1/en
Application granted granted Critical
Publication of EP0775107B1 publication Critical patent/EP0775107B1/en
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Expired - Lifetime legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C251/00Compounds containing nitrogen atoms doubly-bound to a carbon skeleton
    • C07C251/32Oximes
    • C07C251/50Oximes having oxygen atoms of oxyimino groups bound to carbon atoms of substituted hydrocarbon radicals
    • C07C251/54Oximes having oxygen atoms of oxyimino groups bound to carbon atoms of substituted hydrocarbon radicals of hydrocarbon radicals substituted by singly-bound oxygen atoms
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C249/00Preparation of compounds containing nitrogen atoms doubly-bound to a carbon skeleton
    • C07C249/04Preparation of compounds containing nitrogen atoms doubly-bound to a carbon skeleton of oximes
    • C07C249/12Preparation of compounds containing nitrogen atoms doubly-bound to a carbon skeleton of oximes by reactions not involving the formation of oxyimino groups

Definitions

  • the present invention relates to a process for the preparation of O-(2-hydroxyalkyl)oximes of the general formula I in which R 1 and R 2 each stand for an alkyl group having from 1 to 10 carbon atoms, or form, together with the carbon atom to which they are attached, a 5-membered to 7-membered cycloalkyl radical, and R 3 denotes an alkyl group having from 1 to 10 carbon atoms.
  • O-(2-hydroxyalkyl)oximes have great significance as intermediates for plant protectants (cf eg, the prior German Application DE-A 44 15 887).
  • aldoximes and ketoximes with unsubstituted or C 1 -C 8 -alkyl-substituted ethylene or propylene carbonate can be hydroxyalkylated in the presence of catalytic amounts of an N-alkylated, stable organic base or of pyridine substituted by a secondary amine.
  • Preferred process products I are those which can be produced by this process variant those are preferred in which R 1 and R 2 stand for C 1 -C 4 alkyl groups and primarily C 1 -C 3 alkyl groups or form, together with the carbon atom to which they are attached, a cyclopentyl or cyclohexyl ring, and in particular those in which R 1 and R 2 stand for methyl and/or ethyl or form, together with the carbon atom to which they are attached, cyclohexyl.
  • R 3 preferably stands for a C 1 -C 4 alkyl group, particularly for ethyl and more particularly for methyl.
  • Most particularly preferred compounds I are those in which R 1 , R 2 and R 3 stand for methyl.
  • ketoximes II are generally known or are obtainable by known methods, for example, by the reaction of the corresponding ketones with hydroxylamine.
  • the carbonates III are also generally known or can be produced by known methods (cf. eg, EP-A 543,249).
  • the molar ratio of carbonate III to ketoxime II is usually from 1:1 to 10:1 and in particular from 4:1 to 7:1.
  • Suitable catalysts used either alone or in the form of a mixture, are
  • Preferred catalysts are those which are mentioned under ( ⁇ ) and ( ⁇ ).
  • the potassium salts are preferably used, especially potassium fluoride or potassium hydrogen carbonate.
  • the catalyst primarily the inorganic alkali metal salts and the alkali metal salts of carboxylic acids, can be bonded to a support, if desired.
  • suitable supports are aluminum oxide, silica gel, and kieselguhr.
  • the amount of catalyst in these supported catalysts is usually from 10 to 50 wt%.
  • the catalysts are usually employed in an amount of from 5 to 50 mol%, preferably from 5 to 30 mol%, and more preferably from 5 to 10 mol%, based on the ketoxime II.
  • the reaction can be carried out in a single, preferably aprotic, organic solvent or in a solvent mixture. However, the process is preferably carried out without the use of a solvent, in which case an excess of the carbonate III can, in particular, serve as reaction medium.
  • Suitable solvents are for example alkylbenzenes, such as, in particular, toluene and also the xylenes, furthermore dialkylketones such as methyl ethyl ketone, halobenzenes such as chlorobenzene, and ethers such as 1,4-dioxane.
  • the amount of solvent used is usually from 1 to 9 times and in particular from 2 to 7 times the weight of the ketoxime II. lf the amount of solvent exceeds 9 times the weight of the ketoxime II, conversion and yield usually fall.
  • the reaction is preferably carried out at temperatures of from 80°C to 150°C and mostly from 100°C to 140°C and pressures of from 0.5 to 1 bar and especially under standard pressure.
  • phase transfer catalyst usually leads to an increase in reaction rate and conversion. However, for simple processing, it is preferred not to use a phase transfer catalyst.
  • phase transfer catalysts are quaternary ammonium or phosphonium salts, preferably tetraalkylammonium, tetraalkylphosphonium, trialkylbenzylammonium, or trialkylbenzylphosphonium salts, especially triethylammonium, tributylbenzylammonium, and tetrabutylammonium chlorides, bromides, and hydrogen sulfates, and also tributylhexaphosphonium bromide.
  • quaternary ammonium or phosphonium salts preferably tetraalkylammonium, tetraalkylphosphonium, trialkylbenzylammonium, or trialkylbenzylphosphonium salts, especially triethylammonium, tributylbenzylammonium, and tetrabutylammonium chlorides, bromides, and hydrogen sulfates, and also tributylhexaphospho
  • the phase transfer catalyst is usually employed in an amount of from 0.5 to 2 mol% and preferably from 0.7 to 1 mol%, based on the ketoxime II.
  • the reaction can be carried out batchwise or, preferably, continuously.
  • reaction times are normally from 8 to 24 h but mostly from 8 to 16 h.
  • reaction product I takes place by methods known per se, preferably by distillation.
  • the distillation residues of the crude mixture contain substantially unconverted carbonate III and the catalyst.
  • the process is carried out by replenishing the ketoxime II and the carbonate III at a rate equal to the rate of consumption thereof, following the destillation of the product I from the reaction mixture, and the reaction is then repeated.
  • the reaction frequently also produces, as by-product, the regio-isomeric compound Ia which is usually obtained in amounts of up to 10 %, based on I.
  • the two isomeric compounds I and Ia are normally the first overheads occurring during distillation of the crude product. lf desired, the isomer Ia can be substantially separated from the compound I by methods known per se, preferably by fractional distillation.
  • the end products I are important intermediates for crop protection agents, especially for herbicides of the cyclohexenone type (cf. DE-A 44 15 887).

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Medicinal Preparation (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)
  • Catalysts (AREA)
EP95930419A 1994-08-02 1995-07-28 Preparation of o-(2-hydroxyalkyl) oximes Expired - Lifetime EP0775107B1 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE4427289 1994-08-02
DE4427289 1994-08-02
PCT/EP1995/003001 WO1996004238A1 (en) 1994-08-02 1995-07-28 Preparation of o-(2-hydroxyalkyl) oximes

Publications (2)

Publication Number Publication Date
EP0775107A1 EP0775107A1 (en) 1997-05-28
EP0775107B1 true EP0775107B1 (en) 1999-10-13

Family

ID=6524699

Family Applications (1)

Application Number Title Priority Date Filing Date
EP95930419A Expired - Lifetime EP0775107B1 (en) 1994-08-02 1995-07-28 Preparation of o-(2-hydroxyalkyl) oximes

Country Status (17)

Country Link
EP (1) EP0775107B1 (enExample)
JP (1) JP4017022B2 (enExample)
KR (1) KR100388882B1 (enExample)
CN (1) CN1086383C (enExample)
AT (1) ATE185553T1 (enExample)
AU (1) AU3381395A (enExample)
BR (1) BR9508498A (enExample)
CA (1) CA2196452A1 (enExample)
DE (1) DE69512786T2 (enExample)
DK (1) DK0775107T3 (enExample)
ES (1) ES2139935T3 (enExample)
GR (1) GR3031531T3 (enExample)
HU (1) HU216742B (enExample)
IL (1) IL114776A (enExample)
MX (1) MX9700809A (enExample)
WO (1) WO1996004238A1 (enExample)
ZA (1) ZA956402B (enExample)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2000078710A1 (en) * 1999-06-23 2000-12-28 Alliedsignal Inc. Method of making hydroxylamine salts
CN107531617B (zh) * 2015-05-22 2020-10-02 日产化学工业株式会社 O-[1-(2-羟基丙基)]肟化合物的制造方法

Family Cites Families (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3965177A (en) * 1972-05-03 1976-06-22 Texaco Inc. Catalytic process
US5434306A (en) * 1993-11-25 1995-07-18 Ciba-Geigy Corporation Process for the preparation of O-substituted oximes

Also Published As

Publication number Publication date
HUT77753A (hu) 1998-07-28
HU216742B (hu) 1999-08-30
WO1996004238A1 (en) 1996-02-15
DE69512786T2 (de) 2000-03-02
KR100388882B1 (ko) 2004-03-31
JP4017022B2 (ja) 2007-12-05
ZA956402B (en) 1997-02-03
MX9700809A (es) 1997-05-31
KR970704671A (ko) 1997-09-06
CA2196452A1 (en) 1996-02-15
ES2139935T3 (es) 2000-02-16
CN1156445A (zh) 1997-08-06
AU3381395A (en) 1996-03-04
DK0775107T3 (da) 1999-12-27
EP0775107A1 (en) 1997-05-28
BR9508498A (pt) 1997-12-30
CN1086383C (zh) 2002-06-19
JPH10506617A (ja) 1998-06-30
IL114776A (en) 2000-11-21
GR3031531T3 (en) 2000-01-31
ATE185553T1 (de) 1999-10-15
IL114776A0 (en) 1995-11-27
DE69512786D1 (de) 1999-11-18

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